We apply high resolution scanning tunneling microscopy to study intrinsic defect states of bulk FeSe. Four types of intrinsic defects including the type I dumbbell, type II dumbbell, top-layer Se vacancy and inner-layer Se-site defect are extensively analyzed by scanning tunneling spectroscopy. From characterized depression and enhancement of density of states measured in a large energy range, the type I dumbbell and type II dumbbell are determined to be the Fe vacancy and Se$_\mathrm{Fe}$ defect, respectively. The top-layer Se vacancy and possible inner-layer Se-site vacancy are also determined by spectroscopy analysis. The determination of defects are compared and largely confirmed in the annular dark-field scanning transmission electron microscopy measurement of the exfoliated FeSe. The detailed mapping of defect states in our experiment lays the foundation for a comparison with complex theoretical calculations in the future.
Interface-enhanced high-temperature superconductivity in one unit-cell (UC) FeSe films on SrTiO3(001) (STO) substrate has recently attracted much attention in condensed matter physics and material science. By combined in-situ scanning tunneling microscopy/spectroscopy (STM/STS) and ex-situ scanning transmission electron microscopy (STEM) studies, we report on atomically resolved structure including both lattice constants and actual atomic positions of the FeSe/STO interface under both non-superconducting and superconducting states. We observed TiO2 double layers (DLs) and significant atomic di…
Single-layer FeSe film on SrTiO3(001) was recently found to be the champion of interfacial superconducting systems, with a much enhanced superconductivity than the bulk iron-based superconductors. Its superconducting mechanism is of great interest. Although the film has a simple Fermi surface topology, its pairing symmetry is unsettled. Here by using low-temperature scanning tunneling microscopy (STM), we systematically investigated the superconductivity of single-layer FeSe/SrTiO3(001) films. We observed fully gapped tunneling spectrum and magnetic vortex lattice in the film. Quasi-particle i…
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 properties of iron-based superconductors (Fe-SCs) can be varied dramatically with the introduction of dopants and atomic defects. As a pressing example, FeSe, parent phase of the highest-$T_c$ Fe-SC, exhibits prevalent defects with atomic-scale "dumbbell" signatures as imaged by scanning tunneling microscopy (STM). These defects spoil superconductivity when their concentration exceeds 2.5%. Resolving their chemical identity is prerequisite to applications such as nanoscale patterning of superconducting/nonsuperconducting regions in FeSe, as well as fundamental questions such as the mechani…
Cryogenic scanning tunneling microscopy is employed to investigate the stoichiometry and defects of epitaxial FeSe thin films on SrTiO3(001) substrates under various post-growth annealing conditions. Low-temperature annealing with an excess supply of Se leads to formation of Fe vacancies and superstructures, accompanied by a superconductivity (metal)-to-insulator transition in FeSe films. By contrast, high-temperature annealing could eliminate the Fe vacancies and superstructures, and thus recover the high-temperature superconducting phase of monolayer FeSe films. We also observe multilayer Fe…
We used STM to study the tunneling spectra of FeSe0.3Te0.7 films with two orientations of ab-planes and the connection ramp between them. We have discovered that, using pulse laser deposition (PLD) method, the a- and b-axis of the FeSe0.3Te0.7 film deposited on Ar-ion-milled Magnesium Oxide (MgO) substrate are rotated 45 degree with respect to those of MgO, while the a- and b-axis of the film grown on pristine MgO substrate are parallel to those of MgO. With photolithography and this technique, we can prepare FeSe0.3Te0.7 film with two kinds of orientations on the same MgO substrate, and the c…
We report on muon-spin rotation/relaxation (\muSR), electrical resistivity, magnetization and differential scanning calorimetry measurements performed on a high-quality single crystal of Cs_0.8(FeSe_0.98)_2. Whereas our transport and magnetization data confirm the bulk character of the superconducting state below T_c = 28.5(2)K, the \muSR data indicate that the system is {\it magnetic} below T_N = 478.5(3)K, where a first-order transition occurs. The first-order character of the magnetic transition is confirmed by differential scanning calorimetry data. Taken all together, these data indicate …
The work describes the capabilities of Laser Scanning Microscopy (LSM) as a spatially resolved method of testing high_Tc materials and devices. The earlier results obtained by the authors are briefly reviewed. Some novel applications of the LSM are illustrated, including imaging the HTS responses in rf mode, probing the superconducting properties of HTS single crystals, development of twobeam laser scanning microscopy. The existence of the phase slip lines mechanism of resistivity in HTS materials is proven by LSM imaging.
The structural and electronic properties of FeSe ultra-thin layers on Bi$_{2}$Se$_{3}$ have been investigated with a combination of scanning tunneling microscopy and spectroscopy and angle-resolved photoemission spectroscopy. The FeSe multi-layers, which are predominantly 3-5 monolayers (ML) thick, exhibit a hole pocket-like electron band at \barΓ and a dumbbell-like feature at \bar{M}, similar to multi-layers of FeSe on SrTiO$_{3}$. Moreover, the topological state of the Bi2Se3 is preserved beneath the FeSe layer, as indicated by a heavily \it{n}-doped Dirac cone. Low temperature STS does not…
Combining the recent scanning tunneling microscopy (STM) and angle-resolved photoemission spectroscopy (ARPES) measurements, we construct a tight-binding model suitable for describing the band structure of monolayer FeSe grown on SrTiO$_{3}$. Then we propose a possible pairing function, which can well describe the gap anisotropy observed by ARPES and has a hidden sign-changing characteristic. At last, as a test of this pairing function we further study the nonmagnetic impurity-induced bound states, to be verified by future STM experiments.
We prepared single unit cell FeSe films on GaO$_{2-δ}$ terminated perovskite NdGaO$_{3}$(110) substrates and performed ex situ transport and scanning transmission electron microscopy measurements on the FeTe protected films. Our experimental measurements showed that the single unit cell FeSe films interfaced with GaO$_{2-δ}$ layer are electron doped via interface charge transfer. Most importantly, this type of heterostructure can host interface enhanced superconductivity with an onset temperature of about 28 K, which is much higher than the value of 8 K in bulk FeSe. Our work indicates that Fe…
In the recent work by Song et al. [Science 332, 1410 (2011)], the scanning tunneling spectroscopy experiment in the stoichiometric FeSe reveals evidence for nodal superconductivity and strong anisotropy. The nodal structure can be explained with the extended s-wave pairing structure with the mixture of the $s_{x^2+y^2}$ and $s_{x^2y^2}$ pairing symmetries. We calculate the anisotropic vortex structure by using the self-consistent Bogoliubov-de Gennes mean-field theory. In considering the absence of magnetic ordering in the FeSe at the ambient pressure, orbital ordering is introduced, which bre…
The single-layer FeSe films grown on SrTiO3 (STO) substrates have attracted much attention because of its record high superconducting critical temperature (Tc). It is usually believed that the composition of the epitaxially grown single-layer FeSe/STO films is stoichiometric, i.e., the ratio of Fe and Se is 1:1. Here we report the identification of a large amount of excess Fe in the superconducting single-layer FeSe/STO films. By depositing Se onto the superconducting single-layer FeSe/STO films, we find by in situ scanning tunneling microscopy (STM) the formation of the second-layer FeSe isla…
Determination of the pairing symmetry in monolayer FeSe films on SrTiO3 is a requisite for understanding the high superconducting transition temperature in this system, which has attracted intense theoretical and experimental studies but remains controversial. Here, by introducing several types of point defects in FeSe monolayer films, we conduct a systematic investigation on the impurity-induced electronic states by spatially resolved scanning tunneling spectroscopy. Ranging from surface adsorption, chemical substitution to intrinsic structural modification, these defects generate a variety o…
Determining the pairing symmetry of single-layer FeSe on SrTiO$_3$ is the key to understanding the enhanced pairing mechanism; furthermore, it guides exploring new superconductors with high transition temperatures ($T_\mathrm{c}$). Despite significant efforts, it remains controversial whether the symmetry is the sign-preserving $s$- or the sign-changed $s_{\pm}$-wave. Here, we investigate the pairing symmetry of single-layer FeSe from a topological point of view. Using low-temperature scanning tunneling microscopy/spectroscopy, we have systematically characterized the superconducting states at…
We demonstrate the combination of scanning force microscopy and scanning tunneling spectroscopy in a local probe microscope operating at very low temperature (60 mK). This local probe uses a quartz tuning fork ensuring high tunnel junction stability. We performed the spatially-resolved spectroscopic study of a superconducting nano-circuit patterned on an insulating substrate. Significant deviations from the BCS prediction are observed.
The single-layer FeSe/SrTiO3 (FeSe/STO) films have attracted much attention because of their simple crystal structure, distinct electronic structure and record high superconducting transition temperature (Tc). The origin of the dramatic Tc enhancement in single-layer FeSe/STO films and the dichotomy of superconductivity between single-layer and multiple-layer FeSe/STO films are still under debate. Here we report a comprehensive high resolution angle-resolved photoemission spectroscopy and scanning tunneling microscopy/spectroscopy measurements on the electronic structure evolution with doping …
Alkali-metal (potassium) adsorption on FeSe thin films with thickness from two unit cells (UC) to 4-UC on SrTiO3 grown by molecular beam epitaxy is investigated with a low-temperature scanning tunneling microscope. At appropriate potassium coverage (0.2-0.3 monolayer), the tunneling spectra of the films all exhibit a superconducting-like gap larger than 11 meV (five times the gap value of bulk FeSe), and two distinct features of characteristic phonon modes at 11 meV and 21 meV. The results reveal the critical role of the interface enhanced electron-phonon coupling for possible high temperature…
We demonstrate that the differential conductance, $dI/dV$, measured via spectroscopic imaging scanning tunneling microscopy in the doped iron chalcogenide FeSe$_{0.45}$Te$_{0.55}$, possesses a series of characteristic features that allow one to extract the orbital structure of the superconducting gaps. This yields nearly isotropic superconducting gaps on the two hole-like Fermi surfaces, and a strongly anisotropic gap on the electron-like Fermi surface. Moreover, we show that the pinning of nematic fluctuations by defects can give rise to a dumbbell-like spatial structure of the induced impuri…
We investigate the magnetic field distribution near the surface of a magnetic superconductor when a magnetic source is placed close to the superconductor. The magnetic field distribution can be measured by magnetic force microscopy and scanning SQUID microscopy, from which one can extract both the penetration depth $λ_L$ and magnetic susceptibility $χ$. When the magnetic moments are parallel to the surface, one extracts $λ_L/\sqrt{1-4πχ}$. When the moments are perpendicular to the surface, one obtains $λ_L$. By changing the orientation of the crystal, one thus is able to extract both $χ$ and $…
We use scanning tunneling spectroscopy to investigate the filled and empty electronic states of superconducting single-unit-cell FeSe deposited on SrTiO$_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…
Scanning tunneling microscopy can provide a probe for the detailed study of quasiparticle states in high-Tc superconductors. We propose that it can also be used to acquire specific information about impurity-induced quasiparticle states and the superconducting order-parameter structure. In particular, the local density of states is found to be sensitive to impurity-induced resonances and to the symmetry of the order parameter.
In type-1.5 superconductors, vortices emerge in clusters, which grow in size with increasing magnetic field. These novel vortex clusters and their field dependence are directly visualized by scanning SQUID microscopy at very low vortex densities in MgB2 single crystals. Our observations are elucidated by simulations based on a two-gap Ginzburg-Landau theory in the type-1.5 regime.
We propose a set of scanning tunneling microscopy experiments in which the surface of superconductor is scanned by a superconducting tip. Potential capabilities of such experimental setup are discussed. Most important anticipated results of such an experiment include the position-resolved measurement of the superconducting order parameter and the possibility to determine the nature of the secondary component of the order parameter at the surface. The theoretical description based on the tunneling Hamiltonian formalism is presented.
Experimental evidence suggests that FeSe is close to a magnetic instability, and recent scanning tunneling microscopy (STM) measurements on FeSe multilayer films have revealed stripe order locally pinned near defect sites. Motivated by these findings, we perform a theoretical study of locally induced magnetic order near nonmagnetic impurities in a model relevant for FeSe. We find that relatively weak repulsive impurities indeed are capable of generating short-range magnetism, and explain the driving mechanism for the local order by resonant eg-orbital states. In addition, we investigate the im…
Low-temperature scanning tunneling microscopy and spectroscopy are employed to investigate twin boundaries in stoichiometric FeSe films grown by molecular beam epitaxy. Twin boundaries can be unambiguously identified by imaging the 90° change in the orientation of local electronic dimers from Fe site impurities on either side. Twin boundaries run at approximately 45° to the Fe-Fe bond directions, and noticeably suppress the superconducting gap, in contrast with the recent experimental and theoretical findings in other iron pnictides. Furthermore, vortices appear to accumulate on twin boundarie…
Bridging atomic and mesoscopic length scales with Replica Scanning Tunneling Microscopy: Visualizing the atomic lattice of UTe$_2$ and the atomic scale superconducting gap modulations of FeSe close to micron length scales
Universidad Autónoma de Madrid（马德里自治大学）；Universidad del Rosario（罗萨里奥大学）
In this review I discuss the application of scanning magnetic imaging to fundamental studies of superconductors, concentrating on three scanning magnetic microscopies - scanning SQUID microscopy (SSM), scanning Hall bar microscopy (SHM), and magnetic force microscopy (MFM). I briefly discuss the history, sensitivity, spatial resolution, invasiveness, and potential future developments of each technique. I then discuss a selection of applications of these microscopies.
Using low-temperature scanning tunneling microscopy (STM), we studied the vortex states of single-layer FeSe film on SrTiO3 (100) substrate, and the local behaviors of superconductivity at sample boundaries. We clearly observed multiple discrete Caroli-de Gennes-Matricon (CdGM) states in the vortex core, and quantitative analysis shows their energies well follow the formula: E = μΔ^2/E_F, where μ is a half integer and Δ is the mean superconducting gap over the Fermi surface. Meanwhile, a fully gapped spectrum without states near zero bias is observed at [110](Fe) oriented boundary of 1 ML and …
We report an in situ scanning tunneling spectroscopy study of one-unit-cell (1-UC) FeSe film on SrTiO3(001) (STO) substrate. In quasiparticle density of states, bosonic excitation mode characterized by the "dip-hump" structure is detected outside the larger superconducting gap with energy comparable with phonon and spin resonance modes in heavily electron-doped iron selenides. Statistically, the excitation mode, which is intimately correlated with superconductivity, shows an anticorrelation with pairing strength and yields an energy scale upper-bounded by twice the superconducting gap coincidi…
We use scanning tunneling microscopy (STM) and quasiparticle interference (QPI) imaging to investigate the low-energy orbital texture of single-layer FeSe/SrTiO$_3$. We develop a $T$-matrix model of multi-orbital QPI to disentangle scattering intensities from Fe $3d_{xz}$ and $3d_{yz}$ bands, enabling the use of STM as a nanoscale detection tool of nematicity. By sampling multiple spatial regions of a single-layer FeSe/SrTiO$_3$ film, we quantitatively exclude static $xz/yz$ orbital ordering with domain size larger than $δr^2$ = 20 nm $\times$ 20 nm, $xz/yz$ Fermi wave vector difference larger…
We present scanning tunneling microscopy and spectroscopy measurements on a cleaved surface of the LaO0.9F0.1BiSe2 single crystals. Tunneling spectra show a finite local density of states at EF, which is consistent with metallic conductivity in bulk. In addition, the existence of the supermodulation running along the diagonal directions of Bi square lattice was revealed. The period of the supermodulation was about 3 to 5 times the length of the lattice constant. This period is close to that observed in LaO0.5F0.5BiSe2.
We present very low temperature (0.15 K) scanning tunneling microscopy and spectroscopy experiments in the layered superconductor LaSb$_2$. We obtain topographic microscopy images with surfaces showing hexagonal and square atomic size patterns, and observe in the tunneling conductance a superconducting gap. We find well defined quasiparticle peaks located at a bias voltage comparable to the weak coupling s-wave BCS expected gap value (0.17 meV). The amount of states at the Fermi level is however large and the curves are significantly broadened. We find T$_c$ of 1.2 K by following the tunneling…
The search for topological phases of matter is evolving towards strongly interacting systems, including magnets and superconductors, where exotic effects emerge from the quantum-level interplay between geometry, correlation and topology. Over the past decade or so, scanning tunnelling microscopy has become a powerful tool to probe and discover emergent topological matter, because of its unprecedented spatial resolution, high-precision electronic detection and magnetic tunability. Scanning tunnelling microscopy can be used to probe various topological phenomena, as well as complement results fr…
We present a theory for the differential shot noise, $dS/dV$, as measured via shot-noise scanning tunneling spectroscopy, and the differential conductance, $dI/dV$, for tunneling into Majorana zero modes (MZMs) in the putative topological superconductor FeSe$_{0.45}$Te$_{0.55}$. We demonstrate that for tunneling into chiral Majorana edge modes near domain walls, as well as MZMs localized in vortex cores and at the end of defect lines, $dS/dV$ vanishes whenever $dI/dV$ reaches a quantized value proportional to the quantum of conductance. These results are independent of the particular orbital t…
We prepare single layer potassium-doped iron selenide (110) film by molecular beam expitaxy. Such a single layer film can be viewed as a two-dimensional system composed of weakly coupled two-leg iron ladders. Scanning tunneling spectroscopy reveals that superconductivity is developed in this two-leg ladder system. The superconducting gap is similar to that of the multi-layer films. However, the Fermi surface topology given by first-principles calculation is remarkably different from that of the bulk materials. Our results suggest that superconducting pairing is very short-ranged or takes place…
Recently, it has been shown that large stacks of intrinsic Josephson junctions in Bi2Sr2CaCu2O8 emit synchronous THz radiation, the synchronization presumably triggered by a cavity resonance. To investigate this effect we use Low Temperature Scanning Laser Microscopy to image electric field distributions. Apart from verifying the appearance of cavity modes at low bias we find that, in a high input power regime, standing-wave patterns are created through interactions with a hot spot, possibly pointing to a new mode of generating synchronized radiation in intrinsic Josephson junction stacks.
High--quality single crystals of the heavy fermion superconductors CeCoIn$_5$ and CeIrIn$_5$ have been studied by means of low--temperature Scanning Tunneling Microscopy. Methods were established to facilitate \textit{in-situ} sample cleaving. Spectroscopy in CeCoIn$_5$ reveals a gap which persists to above $T_c$, possibly evidencing a precursor state to SC. Atomically resolved topographs show a rearrangement of the atoms at the crystal surface. This modification at the surface might influence the surface properties as detected by tunneling spectroscopy.
Fourier transformation of atomically resolved STM topography of $(LaSe)_{1.14}(NbSe_2)$ revealed a surface modulation along the hexagonal surface lattice of $NbSe_2$ layer, but with a two times larger period. We compare it to the modified charge density wave found on plain $NbSe_2$ under strain.
In this paper we present scanning tunneling microscopy of a large $\textrm{Bi}_2\textrm{Se}_3$ crystal with superconducting PbBi islands deposited on the surface. Local density of states measurements are consistent with induced superconductivity in the topological surface state with a coherence length of order 540 nm. At energies above the gap the density of states exhibits oscillations due to scattering caused by a nonuniform order parameter. Strikingly, the spectra taken on islands also display similar oscillations along with traces of the Dirac cone, suggesting an inverse topological proxim…
